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@ARTICLE{Jovanovic:907825,
      author       = {Jovanovic, Sven and Riegger, Luise M. and Otto, Svenja-K.
                      and Sadowski, Marcel and Kötz, Olaf and Harm, Sascha and
                      Balzat, Lucas G. and Merz, Steffen and Burkhardt, Simon and
                      Richter, Felix H. and Sann, Joachim and Eichel, Rüdiger-A.
                      and Lotsch, Bettina V. and Granwehr, Josef and Albe, Karsten
                      and Janek, Jürgen},
      title        = {{I}nstability of the {L}i7{S}i{PS}8 {S}olid {E}lectrolyte
                      at the {L}ithium {M}etal {A}node and {I}nterphase
                      {F}ormation},
      journal      = {Chemistry of materials},
      volume       = {34},
      number       = {8},
      issn         = {0897-4756},
      address      = {Washington, DC},
      publisher    = {American Chemical Society},
      reportid     = {FZJ-2022-02236},
      pages        = {3659 - 3669},
      year         = {2022},
      abstract     = {Thiophosphate solid electrolytes containing metalloid ions
                      such as silicon or germanium show a very high lithium-ion
                      conductivity and the potential to enable solid-state
                      batteries (SSBs). While the lithium metal anode (LMA) is
                      necessary to achieve specific energies competitive with
                      liquid lithium-ion batteries (LIBs), it is also well known
                      that most of the metalloid ions used in promising
                      thiophosphate solid electrolytes are reduced in contact with
                      an LMA. This reduction reaction and its products formed at
                      the solid electrolyte|LMA interface can compromise the
                      performance of an SSB due to impedance growth. To study the
                      reduction of these metalloid ions and their impact more
                      closely, we used the recently synthesized Li7SiPS8 as a
                      member of the tetragonal Li10GeP2S12 (LGPS) family.
                      Stripping/plating experiments and the temporal evolution of
                      the impedance of symmetric Li|Li7SiPS8|Li transference cells
                      show a severe increase in cell resistance. We characterize
                      the reduction of Li7SiPS8 after lithium deposition with in
                      situ X-ray photoelectron spectroscopy, time-of-flight
                      secondary-ion mass spectrometry, and solid-state nuclear
                      magnetic resonance spectroscopy. The results indicate a
                      continuous reaction without the formation of elemental
                      silicon. For elucidating the reaction pathways, density
                      functional theory calculations are conducted followed by ab
                      initio molecular dynamics simulations to study the interface
                      evolution at finite temperature. The resulting electronic
                      density of states confirms that no elemental silicon is
                      formed during the decomposition. Our study reveals that
                      Li7SiPS8 cannot be used in direct contact with the LMA, even
                      though it is a promising candidate as both a separator and a
                      catholyte material in SSBs.},
      cin          = {IEK-9},
      ddc          = {540},
      cid          = {I:(DE-Juel1)IEK-9-20110218},
      pnm          = {1223 - Batteries in Application (POF4-122) /
                      FestBatt-Charakterisierung - Methodenplattform
                      'Charakterisierung' im Rahmen des Kompetenzclusters für
                      Festkörperbatterien (13XP0176B)},
      pid          = {G:(DE-HGF)POF4-1223 / G:(BMBF)13XP0176B},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000795962300007},
      doi          = {10.1021/acs.chemmater.1c04302},
      url          = {https://juser.fz-juelich.de/record/907825},
}